2nd FEZA School On Zeolites 1

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Transcript 2nd FEZA School On Zeolites 1

Slide 1

2nd FEZA School On Zeolites
1-2 September 2008 , Paris

X-ray photoelectron spectroscopy
and its use for solid materials

Jacques C. Védrine



Slide 2

General scheme representing
different surface techniques
AES: Auger electron spectroscopy
ISS: Ion scattering
spectroscopy SIMS: Secondary ion mass
spectrometry

ions

electrons

photons

ISS

SIMS

AES

XPS, UPS
XAES


Slide 3

Principle of surface techniques
analyser
source of
photons
ions gun
hn

hn

eions

sample

ions


Slide 4

Electron distribution for a given element: 1s2 2s2 2p6 3s2
Transition time10-7 s; Life time of the hole: 10-5 s

hn = Ek + Eb + Fsp


Slide 5

Scheme of XPS electron level energy
Sample

hn = Ek + Eb + Fsp


Slide 6

XPS spectrum taken at photon energies:
1,486.6 eV (AlKa) and 3,000 eV
O KLL
Ce 3d

AlK

Tb 3d

Ce MNN

a

O 1s

Cu 2p

Tb 4d
Ce 4d

3000 eV

1600

1400

1200

1000

800

Binding energy (eV)

600

400

200

0


Slide 7

Illustrative scheme (left) and VG ESCALAB MkII
spectrometer (right)


Slide 8

Main parameters determined by XPS
1. Binding energy values Eb and chemical shifts DEb
(spin-orbit coupling, final state and multielectronic
effects); Auger peaks
2. Quantitative aspects and surface analysis
3. Case of supported catalysts
4. Applications in heterogeneous catalysis: porous
materials, bimetallic catalysts, organometallic
compounds, mixed oxides materials, basic
catalysts, mixed oxides on CeO2, lanthanide
phosphates, adsorbed species,


Slide 9

Chemical shifts corresponding to different
oxidation states and environments of Al
Ni 3p

J=L+S

Al0

Al 2p

S= ½ L= 0,1,2,3
for s,p,d,f orbitals

Al2O3
spin-orbit coupling varies as Z5

Two components with 2J+1 relative intensities

80

70

60


Slide 10

Chemical shifts observed as a function of oxidation state for several
compounds
EC(A,B) = KC(qA- qB) + VA – VB
KC the overlapping integral between core and valence electrons
qA and qB valence charges of element C in A and B compounds
Element

Electronic
level

Compounds

Chemical shift
/eV

Al

2p

Al0-Al2O3

2.7

Si

2p

Si0-SiO2

4.0

Co

2p3/2

Co0-CoO
Co0-Co3O4

2.1
1.8

Ti

2p3/2

Ti0-TiO
Ti0-Ti2O3
Ti0-TiO2

0.9
3.7
5.1

W

4f7/2

W0-WO2
W0-CrWO4
W0-WO3

1.2
2.6
4.2


Slide 11

XPS Parameters










initial state Ei with N electrons
final state Ef with N-1 electrons
Eb = EfN-1 - EiN and DEb = DEi - DEf
charge potential model: DEi = (e2r/r) + DV
er charge borne by the element
DV change in potential due to neighbouring atoms (e.g. Madelung potential V= Sj
(qj/Rj) Rj distance between C and atom j bearing a charge qj )
KCq = q/ri, with ri average radius of element C
Final state effects (Koopmans theorem of sudden approximation relaxation) Eib = -ei
+ EiR and DEib = -Dei + DEiR
Multielectronic effects: plasmons, configuration interaction, shake-up and shake-off
processes. npligand  nptransition metal difference in energy beween the background state
and the states after photoemission (shake-off if electron ejected in the continuum)
Shake-up peaks for paramagnetic ions as Co2+ (d7), Ni2+ + (d8) or Cu2+ (d9)
Configuration interaction: e.g. Mn2+ d5 ion 6S initial state (Ar 3s23p63d5) and 7S final
state [with two states 7S and 5S depending on the spin orientation] Mn3+ (Ar
3s13p63d5) and energy splitting DE(7S-5S) = [(2S+1)/(2L+1)]G(s,d) [G(s,d) exchange
intergral] and I(7S)/I(5S) = 7/5 as spin-orbit coupling between 2p, 3d, 4f peaks and
(2L+1) /(2S+1) relative peaks intensities.


Slide 12

Principle of the Auger process occurring under photon
or electron impact
e- / photon
e- Auger

e-

Z

Y

X

Ec = E X - EY - EZ

EKL2L3 = EK - EL2 – EL3 – F(L2,L3,X) + R(L2,L3)


Slide 13

Intensity I = P of the emitted beam as a function of its
originating depth x = d from the surface


Slide 14

Universal curve of the electron mean free path
as a function of the electron kinetic energy value

10 eV

100 eV


Slide 15

Quantitative aspects
• dI(q) = F.(NA0/sinq)(ds./d).T.exp(-x/lsinq)dx


• I = I0 ∫0 exp(-xl).d(x) = lI0 [exp(-xl)]0 = lI0

• I(q) = ∫0 F (NA0/sinq)(ds./d).T.exp(-x/lsinq)dx
= FNA0(ds./d).T.l

• NA/NB = (IA/IB)(sB/sA)(TB/TA)(lB/lA)
• (ds/d ).(q,hn) = (s/4p) [1+ (b/2).{(3sin2a)/2)-1}]
• NA/NB = (IA/IB).[sB (EkB)x] / [sA (EkA)x] .TB/TA
with x = 0.5 to 0.75


Slide 16

Scheme of a supported catalyst of high surface area support as proposed
by Kerkhof et al

(Ip/Is)exp = (Np/Ns)b (sp/ss){ [1+ exp(-ds/2ls)] / [1-exp(-ds/2ls)]}{[1-exp(-dp/l p)]
/ (dp/lp}} ds = 2/S.r

1

Support

Promoter

2

j

Ip/IS = (NS/Np).(sp/ss).(ds/2l)

Approx.:
catalyst particle =
infinite number of
sheets
high surface area


Slide 17

Ip/IS = (NS/Np).(sp/ss).F(d,lp)

• F(d,lp) = (3/2).{1-(2lp2/d2)[1-exp(-d/lp)]+ (2
lp/d) exp(-d/lp)} for spherical crystallites of
diameter d
• F(d,lp) = 3{[1-(8lp2/d2)].[1-exp(-d/2lp)] +
(4lp/d) exp(-d/2lp)} for hemispherical
crystallites of diameter d
• F(d,lp) = 1-exp(-d/lp) for cubic or planar
deposits of thickness d


Slide 18

Prediction and experimental metal dispersion for Pt/SiO2
catalysts

0,35

monolayer

0,3

IPt/ISi
monolayer
I Pt/I Si exptl

0,25
0,2
0,15
0,1
0,05
0
0,0E+00

5,0E-03

1,0E-02

Pt/Si bulk

1,5E-02


Slide 19

Schematic models for supported catalysts

1

1

1

2

2

2

3

3

3

a) Layer mode

b) Island mode

c) Layer + island

(Frank-van der
Merwe, 2 D)

(Volmer-Weber, 3 D)

mode
(StranskiKrastanov)

(a)

IS
 d
 exp   
IS0
 l

(f = 0.5)
(b)

IS
 d 
 1  f   f exp   i 
IS0
 l

(c)

IS
 d 
 dm 
 exp  _ 1  f   f exp   i 
IS0
 l 
 l 


Slide 20

IS /IS 0

Theoretical calculated XPS peak intensity ratio
variations for supported catalysts. Case of Cu/MgO
1,2
1
0,8
0,6
0,4
0,2
0

model a
model b
model c

IS /IS 0

0

5

10

1,2
1
0,8
0,6
0,4
0,2
0

15
mean coverage (Å)

model a
model b
model c
Cu/M gO

0

5

10

15
mean coverage (Å)


Slide 21

Ag 3d XPS spectra of 0.3Pd-0.6Ag/pumice catalyst in a)
as synthesised; b) oxidised at 623K; c) reduced at 623K


Slide 22

Spectra of MgNd alloys (25wt% Nd) oxidised for 90 min at 773K


Slide 23

O1s, Eu 3d5/2 and Eu 4d XPS spectra of EuIII
organometallic compounds


Slide 24

Binding energy values in eV of Eu3d5/2 peaks and of its associated
shake-down satellite and ratio of intensities for EuIIIcompounds
EuIIIcompounds
Eu2O3
Eu2 (C2O4)3
Eu(acac)3
Eu2 (CO3)3
Eu2 (SO4)3
Eu(NO3)3

Eb Eu3d5/2

Eb shake down satellite

DEb

1133.7
1133.9
1135.0
1135.3
1135.9
1136.4

1123.5
1124.0
1124.9
1125.2
1125.7
1126.0

10.2
9.9
10.1
10.1
10.2
10.4

For europium 4f65d1and 4f75d0 configurations in the final state
unoccupied 4f levels are lowered in energy by the potential of the
created photohole (Coulomb interaction of the created photohole
with the electron system)


Slide 25

Correlation between Pauling electronegativity of the heteroatom X
and O1s binding energy values for EuIII compounds


Slide 26

Basic oxide catalysts used for propane ODH to propene
Rare earth element Mg, Ca, Sr doped with Nd (5 mol% Nd2O3)
(Nd 3d (left) and Nd 4d (right) core levels from the Nd/CaO

sample; insert: Nd 3d5/2 peak decomposition
34000
Nd 3d3/2

Nd 3d5/2

26000

29000
O KLL Auger line

25000
21000

990

985

980

975

970

965

Intensity (arb. units)

33000

22000
18000

800
600
400
200

145

10000
1000

1000

14000

17000
960

Binding energy (eV)

1020

1200

980

Binding energy (eV)

960

140

135

130
125
Binding energy (eV)

120

115

0
110

Intensity (arb. units)

Nd 3d 5/2

Intensity (arb. units)

30000


Slide 27

Nd content as determined from chemical analysis and XPS
Nd 3d or Nd 4d, M* = Mg 1s, Ca 2p, Sr 3d peak intensities
Catalysts

Nd/M*
Chem Anal.

Nd/M*
XPS

Excess of
Nd on the
surface (at %)

Nd/MgO

0.10

0.17 ± 0.04

5.4

Nd/CaO

0.09

0.14 ± 0.02

4.0

Nd/SrO

0.10

0.13 ± 0.02

2.4

slight enrichment (<5%) of the surface with Nd with respect to the bulk


Slide 28

XPS spectra before catalytic testing and their
decomposition: Nd/MgO (a), Nd/CaO (b), Nd/SrO (c)
55000

23000
19000
15000
11000

538

536

534
532
530
Binding energy (eV)

Intensity (CPS)

a

b

25000
15000

7000
526

528

35000

538

536

534

532

530

528

5000
526

Binding energy (eV)

7000

5000

3000

538

536

534

532

530

528

Intensity (eV)

cc

1000
526

Binding energy (eV)

O1s in oxide (Eb ~ 530.0 eV), in adsorbed water Eb ~ 534.0 eV and from
hydroxyls and carbonates (Eb ~ 532.0 eV),

Intensity (CPS)

45000


Slide 29

C1s XPS peaks before catalytic testing and their
decomposition: Nd/MgO (a), Nd/CaO (b), Nd/SrO (c)
13000
5500

Carbonate

295

290

2500

b
Carbonate

1000
280

295
Carbonate

285

Binding energy (eV)

5000

290

3500

Carbonate
1500

280

270

Intensity (CPS)

Sr 2p1/2
2500

290

285

1000
280

Binding energy (eV)

Sr 2p3/2

c

9000

Intensity (CPS)

4000

Intensity (CPS)

a

500
260

Binding energy (eV)

C1s peaks at ~ 285 eV for contamination carbon (adventitious hydrocarbon
species) and ~ 290.0 eV for carbonates


Slide 30

Mixed oxides based on CeO2
Ce 3d experimental spectrum and its decomposition
Final state effect: v (u)
v’’(u’’):
Multiplet splitting: v’’’(u’’’):
vo(uo):
v’(u’):
u’’’
v’’’
u
u’’

CeIV : 3d95d6s0 4f1-O2p5
CeIV : 3d95d6s0 4f2-O2p4
CeIV : 3d95d6s0 4f0-O2p6
CeIII : 3d95d6s0 4f1-O2p6
CeII : 3d9 5d6s0 4f2-O2p5
v

u’
v’
v’’

910

900

890

918

908

898

880

v0

870

888
878
Binding Energy (eV)


Slide 31

Concluding remarks
• XPS is the most currently used « surface » technique
• Quantitative data are determining but should be used
with care, unless the geometry of particles and
support are well known
• Not really useful for porous materials as too sensitive
to the surface (1-5nm) of particles usually in mm-mm
size range
• Chemical shifts and multiplet peaks are useful
« chemical » indications
• Challenges for analysis under « pressure » and for
spatial resolution and scanning analysis